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The biotemplating technique is an environmental-protective high-efficiency new technology by which the resulting TiO2 may simultaneously attain the duplication of structure and self-doping elements from biotemplate materials, which is highly desirable for photocatalytic applications. In this paper, aquatic plant leaves—including reed, water hyacinth, and duckweed—were used as both templates and silicon precursors to successfully synthesize biomorphic TiO2/SiO2 composite with mesoporous structures. X-ray diffraction, scanning electron microscopy, transmission electron microscopy, N2 adsorption–desorption, and UV–visible diffuse reflectance spectra were applied to characterize the microstructures of the samples. The results show that all TiO2/SiO2 composites are mainly composed of an anatase phase with mesoporous structure and possess high specific surface area. Compared with commercial Degussa P25 TiO2, all TiO2/SiO2 samples display intensive light-harvesting efficiency, particularly in the visible light range. The activities were evaluated by using gentian violet as a target for photocatalytic degradation experiments under simulated solar irradiation. The TiO2/SiO2 samples templated by reed and water hyacinth leaves exhibit high activity, while the TiO2/SiO2 samples obtained from duckweed are inferior to P25 in the degradation of gentian violet. A synergistic effect of SiO2 incorporation and structural construction through biotemplating is proposed to be beneficial to photocatalytic activity.